No abstract

Controlling the propagation and interaction of light in complex media has sparked major interest in the last few years. Unfortunately, spatial light modulation devices suffer from limited speed that precludes real-time applications such as imaging in live tissue. To address this critical problem we introduce a phase-control technique to characterize complex media based on the use of fast 1D spatial light modulators and a 1D-to-2D transformation performed by the same medium being analyzed. We implement the concept using a micro-electro-mechanical grating light valve (GLV) with 1088 degrees of freedom modulated at 350 KHz, enabling unprecedented high-speed wavefront measurements. We continuously measure the transmission matrix, calculate the optimal wavefront and project a focus through various dynamic scattering samples in real-time, all within 2.4 ms per cycle. These results improve prior wavefront shaping modulation speed by more than an order of magnitude and open new opportunities for optical processing using 1D-to-2D transformations.

Time-resolved emission techniques were employed to study the reversible proton photoprotolytic properties of surface-attached 8-hydroxypyrene-1,3,6-trisulfonate (HPTS) molecules to hydrophilic alumina and silica surfaces. We found that the excitedstate proton transfer rate of the surface-linked HPTS molecules, in H 2 O and D 2 O, is nearly the same as of HPTS in the bulk, while the corresponding recombination rate is significantly greater. Using the diffusion-assisted proton geminate-recombination model, we found that the best fit of the time-resolved fluorescence (TRF) signal is obtained by invoking a twodimensional diffusion space for the proton to recombine with the conjugated basic form, RO − *, of the surface-linked HPTS. However, we obtain an excellent fit by a three-dimensional diffusion space for diffusional HPTS in bulk water. These results indicate that the photoejected solvated protons are confined to the surface for long periods of time. We suggest two plausible mechanisms responsible for two-dimensional proton diffusion next to hydrophilic surfaces.

A strong increase of spontaneous radiative emission from colloidally synthesized CdSe/CdS/PMMA hybrid particles is achieved when manipulated into plasmonic bullseye resonators with the tip of an atomic force microscope (AFM). This type of antenna provides a broadband resonance, which may be precisely matched to the exciton ground state energy in the inorganic cores. Statistically analyzing the spectral photoluminescence (PL) of a large number of individual coupled and uncoupled CdSe/CdS/PMMA quantum dots, we find an order of magnitude of intensity enhancement due to the Purcell effect. Time-resolved PL shows a commensurate increase of the spontaneous emission rate with radiative lifetimes below 230 ps for the bright exciton transition. The combination of AFM and PL imaging allows for sub-200 nm localization of the particle position inside the plasmonic antenna. This capability unveils a different coupling behavior of dark excitonic states: even stronger PL enhancement occurs at positions with maximum spatial gradient of the nearfield, effectively adding a dipolar component to original quadrupole transitions. The broadband maximization of light-matter interaction provided by our nanoengineered compound systems enables an attractive class of future experiments in ultrafast quantum optics.

We demonstrate a new, label-free, far-field super-resolution method based on an ultrafast pump-probe scheme oriented toward nanomaterial imaging. A focused pump laser excites a diffraction-limited spatial temperature profile, and the nonlinear changes in reflectance are probed. Enhanced spatial resolution is demonstrated with nanofabricated silicon and vanadium dioxide nanostructures. Using an air objective, resolution of 105 nm was achieved, well beyond the diffraction limit for the pump and probe beams and offering a novel kind of dedicated nanoscopy for materials.